Independent component analysis (ICA) and dictionary learning (DL) are the most successful blind source separation (BSS) methods for functional magnetic resonance imaging (fMRI) data analysis. However, ICA to higher and DL to lower extent may suffer from performance degradation by the presence of anomalous observations in the recovered time courses (TCs) and high overlaps among spatial maps (SMs). This paper addressed both problems using a novel three-layered sparse DL (TLSDL) algorithm that incorporated prior information in the dictionary update process and recovered full-rank outlier-free TCs from highly corrupted measurements. The associated sequential DL model involved factorizing each subject’s data into a multi-subject (MS) dictionary and MS sparse code while imposing a low-rank and a sparse matrix decomposition restriction on the dictionary matrix. It is derived by solving three layers of feature extraction and component estimation. The first and second layers captured brain regions with low and moderate spatial overlaps, respectively. The third layer that segregated regions with significant spatial overlaps solved a sequence of vector decomposition problems using the proximal alternating linearized minimization (PALM) method and solved a decomposition restriction using the alternating directions method (ALM). It learned outlier-free dynamics that integrate spatiotemporal diversities across brains and external information. It differs from existing DL methods owing to its unique optimization model, which incorporates prior knowledge, subject-wise/multi-subject representation matrices, and outlier handling. The TLSDL algorithm was compared with existing dictionary learning algorithms using experimental and synthetic fMRI datasets to verify its performance. Overall, the mean correlation value was found to be 26%\\documentclass[12pt]{minimal} \\usepackage{amsmath} \\usepackage{wasysym} \\usepackage{amsfonts} \\usepackage{amssymb} \\usepackage{amsbsy} \\usepackage{mathrsfs} \\usepackage{upgreek} \\setlength{\\oddsidemargin}{-69pt} \\begin{document}$$26\\%$$\\end{document} higher for the TLSDL than for the state-of-the-art subject-wise sequential DL (swsDL) technique.